Mercury (Hg) concentrations were measured in 394 surface and core samples from Long Island Sound (LIS). The surface sediment Hg concentration data show a wide spread, ranging from <50 ppb Hg in eastern LIS to >600 ppb Hg in westernmost LIS. Part of the observed range is related to variations in the bottom sedimentary environments, with higher Hg concentrations in the muddy depositional areas of central and western LIS. A strong residual trend of higher Hg values to the west remains when the data are normalized to grain size. Relationships between a tracer for sewage effluents (C. perfringens) and Hg concentrations indicate that between 0-50 % of the Hg is derived from sewage sources for most samples from the western and central basins. A higher percentage of sewage-derived Hg is found in samples from the westernmost section of LIS and in some local spots near urban centers. The remainder of the Hg is carried into the Sound with contaminated sediments from the watersheds and a small fraction enters the Sound as in situ atmospheric deposition. The Hg-depth profiles of several cores have well-defined contamination profiles that extend to pre-industrial background values. These data indicate that the Hg levels in the Sound have increased by a factor of 5-6 over the last few centuries, but Hg levels in LIS sediments have declined in modern times by up to 30 %. The concentrations of C. perfringens increased exponentially in the top core sections which had declining Hg concentrations, suggesting a recent decline in Hg fluxes that are unrelated to sewage effluents. The observed spatial and historical trends show Hg fluxes to LIS from sewage effluents, contaminated sediment input from the Connecticut River, point source inputs of strongly contaminated sediment from the Housatonic River, variations in the abundance of Hg carrier phases such as TOC and Fe, and focusing of sediment-bound Hg in association with westward sediment transport within the Sound.